Ferroelectric Polarization-Modulated Interfacial Fine Structures Involving Two-Dimensional Electron Gases in Pb(Zr,Ti)O3/LaAlO3/SrTiO3 Heterostructures.

Interfacial fine structures of bare LaAlO3/SrTiO3 (LAO/STO) heterostructures are compared with those of LAO/STO heterostructures capped with upward-polarized Pb(Zr0.1,Ti0.9)O3 (PZTup) or downward-polarized Pb(Zr0.5,Ti0.5)O3 (PZTdown) overlayers by aberration-corrected scanning transmission electron microscopy experiments. By combining the acquired electron energy-loss spectroscopy mapping, we are able to directly observe electron transfer from Ti4+ to Ti3+ and ionic displacements at the interface of bare LAO/STO and PZTdown/LAO/STO heterostructure unit cell by unit cell. No evidence of Ti3+ is observed at the interface of the PZTup/LAO/STO samples. Furthermore, the confinement of the two-dimensional electron gas (2DEG) at the interface is determined by atomic-column spatial resolution. Compared with the bare LAO/STO interface, the 2DEG density at the LAO/STO interface is enhanced or depressed by the PZTdown or PZTup overlayer, respectively. Our microscopy studies shed light on the mechanism of ferroelectric modulation of interfacial transport at polar/nonpolar oxide heterointerfaces, which may facilitate applications of these materials as nonvolatile memory.